Nuclear Instruments and Methods in Physics Research A 484 (2002) 613–618 Study of the neutron radiography characteristics for the solid state nuclear track detector Makrofol-DE Reynaldo Pugliesi*, Marco A. Stanojev Pereira ! Divisao * de F!ısica NuclearFTFF, Instituto de Pesquisas Energeticas e Nucleares, IPEN/CNEN-SP, Caixa Postal 11.049FPinheiros, CEP 05422-970 Sao * Paulo, SP, Brazil Received 14 June 2001; received in revised form 13 August 2001; accepted 17 August 2001 Abstract In this work, the track-etch method was employed for Neutron Radiography purposes. A combination of the Solid State Nuclear Track Detector Makrofol-DE with a natural boron converter screen has been used to register the image. The radiography characteristics such as, track size, track production rate, characteristic curves and spatial resolution, have been studied. The detectors were irradiated up to neutron exposures about 5 1010 n/cm2, in a radiography facility installed at the IEA-R1 Nuclear Research Reactor, and etched in a KOH aqueous solution at a constant temperature of 701C. The obtained results were compared with those reported by other authors, and discussed according to the theory of the image formation in solid state nuclear track detectors. The experimental conditions to obtain the best image contrast, and the corresponding value of the spatial resolution, were also determined. r 2001 Elsevier Science B.V. All rights reserved. PACS: 81.70; 07.85.Y; 87.59.B Keywords: Radiography; Non destructive testing technique 1. Introduction The solid state nuclear track detectors (SSNTD) are able to register some charged particles by the radiation damage caused along their interaction path in this material. These damages, under an adequate chemical etching, are enlarged and called tracks [1,2]. In the track-etch neutron radiography (NR) method, a test object is usually irradiated in a uniform neutron beam and a converter screen *Corresponding author. E-mail address: [email protected] (R. Pugliesi). transforms the transmitted neutrons into ionizing radiation, able to sensibilize the SSNTD. After chemical etching (development), the resulting tracks will form a two-dimensional image, which is visible by naked eye. The main reasons that makes these detectors attractive for NR purposes are its insensitivity to register visible light, b and g radiations as well as the high intrinsic spatial resolution obtainable in the radiography image. Its main disadvantage is the low optical contrast achieved in the image [3]. The main objective of the present work was to determine the experimental conditions to achieve the best contrast in the image for the SSNTD 0168-9002/01/$ - see front matter r 2001 Elsevier Science B.V. All rights reserved. PII: S 0 1 6 8 - 9 0 0 2 ( 0 1 ) 0 1 9 7 2 - 6 614 R. Pugliesi, M.A. Stanojev Pereira / Nuclear Instruments and Methods in Physics Research A 484 (2002) 613–618 Makrofol-DE, and to discuss its radiography characteristics according to the image formation theory in SSNTD, which is a model based on the optical properties of a single track [3–6]. 3. Results and discussion The following radiography characteristics for the Mk-DE detector were investigated: 3.1. Track size 2. Experimental Table 1 Characteristics of the neutron beam at the irradiation position Neutron flux 3 106 n/s cm2 Collimation ratio (L=D) n=g ratio Beam diameter (Au)–Cd ratio 70 >105 n/cm2 mR 20 cm B150 The image contrast as well as the spatial resolution obtained in the radiography image are usually influenced by the track diameter and so they are etching time dependent. In general, small tracks provide higher contrast and better resolution than the larger ones [3,9,10]. The track diameters have been evaluated as a function of the etching time for a negligible track overlapping condition. In the present work, it was achieved for neutron exposure of about xB9 107 n/cm2. Fig. 1 shows the results of the track diameter behavior as a function of the etching time. Each experimental data has been obtained by averaging the values of 10 distinct tracks, visually determined onto the screen of the microscope TVmonitor system, by using a previously calibrated length scale. The track diameters ranged from 1.4 mmoft o8 mm for etching times varying from 2ote o25 min. According to the data reported in literature, good quality radiographs can be obtained when working with track diameters ft o5 mm. As shown in Fig. 1, for the present detector such diameters can be achieved for etching times te o15 min [7]. track diameter(µm ) The present NR facility is installed at the radial beam-line 08 of the pool type IEA-R1 Nuclear Research Reactor that operates at a power of 2 MW producing a thermal neutron flux of about 1013 n/s cm2 near the reactor core. The main characteristics of the neutron beam at the irradiation position are listed in Table 1 [7]. The SSNTD Makrofol-DE (Mk-DE) is a policarbonate 500 mm thick, manufactured by Bayer AG [8]. The converter screen is a plastic backing, single coated with a natural boron layer having 106 and 65 mm thickness, respectively, produced by Kodak Pathe" French. During irradiation, the detector and the screen are kept in a tight contact inside an aluminum cassette. The damages into the Mk-DE are induced by the products of the nuclear reaction B10(n,a)Li7 (a-energy=1.47 MeV; Li-energy=0.84 MeV) and its intrinsic registration efficiency is near the unity [5]. The chemical etching was performed in a PEW solution (40 g ethanol, 45 g water, 15 g KOH) at a constant temperature of 701C [7]. After chemical etching, the detectors have been analyzed employing two systems. The first one was a Leitz optical microscope (magnification power 1500 ) coupled to a TV-monitor to analyze individual tracks and the second one was a Jarrel-Ash optical microphotometer, having a scanning beam width of 3 mm and length of 700 mm, to analyze light transmission through the detectors. 10 9 8 7 6 5 4 3 2 1 0 0 3 6 9 12 15 18 21 24 etching time(min) Fig. 1. Track diameter as a function of the etching time. R. Pugliesi, M.A. Stanojev Pereira / Nuclear Instruments and Methods in Physics Research A 484 (2002) 613–618 3.2. Track production rate 3.3. Characteristic curve A characteristic curve relates optical density, Dop ; as a function of the neutron exposure. Optical density is defined as ‘‘Dop ¼ logðIo =IÞ’’, where Io 2 track density(tr/cm )x10 6 3 2 1 0 0 5 10 15 20 25 30 35 40 45 etching time(min) Fig. 2. Track density as a function of the etching time. 6 2 track density(tr/cm ) 4x10 6 3x10 6 2x10 6 1x10 0 0 8 2x10 8 4x10 8 6x10 8 8x10 2 neutron exposure(n/cm ) Fig. 3. Track density as a function of neutron exposure for 6 min etching time. 1.4 1.2 optical density This quantity represents the track to neutron conversion efficiency. It was determined for the etching time where the efficiency is maximal. For such purpose one detector has been irradiated at the exposure x ¼ 3 108 n/cm2, and the track density evaluated for several etching times in the interval from 2 to 40 min. Each track density value has been obtained by averaging the amount of tracks counted in 10 distinct areas of the detector foil. The counting was visually performed, onto the screen of the microscope TV-monitor system. Fig. 2 shows the track density behavior as a function of the etching time and the efficiency is maximal for about 6 min. In order to determine the track production rate, the detectors have been irradiated in neutron exposures ranging from 9 107 n=cm2 oxo 8 108 n/cm2 and etched in 6 min. The track density was also determined by visual counting and its behavior as a function of the neutron exposure is shown in Fig. 3. The track production rate was evaluated from the slope of the straight line fitted to the experimental data points, and the obtained value was tr=n¼ ð4:470:1Þ 103 [7]. 615 1.0 0.8 0.6 0.4 0.2 0.0 7 10 8 9 10 10 10 10 2 neutron exposure(n/cm ) Fig. 4. Characteristics curves for three etching times: (’) 2 min; (K) 6 min; (m) 10 min. and I are the intensities of the incident and transmitted light through the detector, respectively. In the present work, light intensity readings have been determined by using the optical microphotometer. Fig. 4 shows the behavior obtained for the optical density as a function of the neutron exposures in the interval from 3 107 n/ cm2oxo6 1010 n/cm2 for three etching times 2, 6 and 10 min. According to the image formation theory, a track can be represented by an inner circle surrounded by an external ring, which is responsible by the darkening of the image, as shown in 616 R. Pugliesi, M.A. Stanojev Pereira / Nuclear Instruments and Methods in Physics Research A 484 (2002) 613–618 Fig. 5. Schematic representation of a single track. practical purposes is usual to employ the mean value of G which is obtained from the slope of the straight line fitted to the steeper region of the characteristic curve [11]. The best value obtained for the image contrast was G ¼ ð1:1070:01Þ for etching times of 6 and 10 min. However, the selected etching time was 6 min because, in this case, the tracks are smaller and the dynamic range is greater [7]. For this etching time the neutron exposure range was 1.8 109 n/cm2oxo 10 2 3 10 n/cm . It was also verified that for these same experimental conditions the fast neutron optical density background, caused by (n; p) reactions is negligible. For such evaluation the detectors have been irradiated without converter screen. 3.4. Resolution Fig. 6. Schematic representation of two overlapped tracks. Fig. 5. When the tracks are overlapped, see Fig. 6, the external ring area will be smaller and consequently the optical density increases is slower. Hence, the behavior of the characteristic curve for etching time te ¼ 6 min can be explained as follows: for neutron exposure up to xB1 109 n/ cm2, the track density is relatively low and, consequently, insufficient to produce appreciable optical density above the detector background (Dop B0:04); between 1 109 n/cm2oxo 10 2 3 10 n/cm , a competition between single track production (responsible for optical density increase) and track overlapping (responsible for optical density decrease) leads to a proportional increase of the optical density. In this case, the first process is overcoming the second one; for x > 3 1010 n/cm2, track overlapping is predominant and the optical density decreases [3]. The optical contrast is defined by ‘‘G ¼ dðDop Þ=dðlog xÞ’’ and its value varies for each point of the characteristic curve [6]. For In radiography, the spatial resolution is defined as the minimum distance that two objects must be separated before they can be distinguished from each other [6]. The resolution is usually quoted in terms of the total unsharpness (Ut ) and results from the combined effect of the intrinsic unsharpness (Ui ) from the detector/converter screen combination and of the geometric unsharpness (Ug ) from the angular divergence of the neutron beam and are related by the empirical equation [12]: ðUt Þn ¼ ðUi Þn þ ðUg Þn ð1Þ where 1ono3: In the present work, the total unsharpness has been obtained by scanning the optical density distribution at the interface between two images: the first one corresponding to a neutron opaque knife edge test object (gadolinium foil 127 mm thick, irradiated in a tight contact with the detector) and the second one corresponding to the direct neutron beam. The following Edge Spread Function-ESF [13,14] was fitted to the resulting distribution: ESF ¼p1 þ p2 arctanðp3 ðX p4 ÞÞ ð2Þ where X is the scanning coordinate and p1 ; p2 ; p3 and p4 ; are free parameters. The total unsharpness is given by ‘‘Ut ¼ 2=ðp3 Þ’’ [13]. 617 R. Pugliesi, M.A. Stanojev Pereira / Nuclear Instruments and Methods in Physics Research A 484 (2002) 613–618 0.6 optical density 0.5 0.4 0.3 0.2 0.1 0 100 200 300 400 500 scann coordinate(µm ) Fig. 7. Optical density distribution for a gadolinium knife edge test object and the fitted Edge Spread Function. Table 2 Values of total unsharpness-Ut as a function of the neutron exposure for etching time 6 min Neutron exposure (n/cm2) Ut (mm) 9 1.8 10 5.4 109 1.0 1010 3.2 1010 2172 2372 2272 3372 30 intrinsic unsharpness(µm ) Since the main disadvantage of the present method is the low optical contrast achieved in the image, the conditions of exposure range and etching times for which the total unsharpness has been evaluated were the same as the ones for which the best image contrast was determined, that is, 1.8 109 n/cm2oxo3 1010 n/cm2 and 6 min, respectively. The light transmission readings were performed by using the same microphotometer and a typical resulting optical density distribution as well as the fitting of the ESF, are shown in Fig. 7. Table 2 gives the obtained results for Ut as a function of the exposure for 6 min etching time. The comparison of the present results with those obtained from the theory of the image formation in SSNTD was performed through the values of the intrinsic unsharpness Ui : This theory states that Ui is independent of the neutron exposure and remains constant at a minimal value ‘‘Ui B0; 8 R’’ (R is the range of the a-particle in the converter screen) for a negligible overlapping condition and for track diameters ft oR: The greater the exposure, the greater the track overlapping and for this condition ‘‘Ui a logðxÞ’’ [6]. Since for the screen used in the present work the RB9 mm, the best value for the intrinsic unsharpness is theoretically Ui B7 mm. For the present radiography facility L=DB70 and since the distance between the gadolinium foil and the converter screen was 630 mm, the contribution of the geometrical unsharpness to the 25 20 15 10 5 0 9 10 10 10 2 neutron exposure(n/cm ) 11 10 Fig. 8. Intrinsic unsharpness behavior as a function of the neutron exposure for etching time 6 min. total one was about Ug B9 mm. By using the values found for Ut and Ug ; the intrinsic unsharpness can be evaluated by means of Eq. (1) with n ¼ 1; 5 [14]. Fig. 8 shows the behavior of Ui as a function of the exposure for 6 min etching time. These values show a very similar trend when compared with the ones obtained from the theory. The values remain approximately constant at about 17 mm up to exposure about xB2 1010 n/cm2 and increase with ‘‘logðxÞ’’ when track overlapping becomes predominant. The discrepancy observed between the best theoretical (7 mm) and experimental (17 mm) values is attributed to the contact irregularities at the detector/screen interface as well as to the neutron beam and screen inhomogeneities. The former leads to an a-particle scattering in the remaining air layer at this interface and the latter to the presence of small track clusters which have been observed by microscope, even at low neutron exposures [7]. 618 R. Pugliesi, M.A. Stanojev Pereira / Nuclear Instruments and Methods in Physics Research A 484 (2002) 613–618 4. Conclusions By taking into account the results obtained in the characterization of the SSNTD Makrofol-DE for NR purposes, the experimental conditions to obtain the best contrast in the radiography image are: 6 min for the etching time and 1.8 109 n/cm2oxo3 1010 n/cm2 for the neutron exposure range. For such conditions the following characteristics were achieved: track diameter 2.570.2 mm; track to neutron conversion efficiency 4.470.1 103, image contrast 1.1070.01; total unsharpness from 2172 to 3372 mm. The obtained results agree with those ones given by the image formation theory for SSNTD which states that the best contrast and spatial resolution are achieved when the image is formed by many small tracks instead by few large ones [3,11]. The main characteristic of the present method is its high intrinsic unsharpness, which theoretically can reach a value of about 7 mm. Although the obtained experimental value is high, about 17 mm, it can be promptly improved by using an evacuated cassette. This characteristic together with its insensitivity to register visible light, b and g radiations, making the method useful for example to obtain high resolution images for high radioactive materials. Table 3 gives comparative data for several NR methods [11,15,16]. Table 3 Comparison of some characteristics for different radiography methods Converter screen Film/ detector Irrad. time (min) Intrinsic unsharpness (mm) Gd Dy B(natural) B(natural) B(natural) Kodak-AA Kodak-AA CN-85 Mk-DE CR-39 5 10 120 120 120 70 400 12 17 13 The main disadvantage of the present method, when compared with the one employing emulsion films, is the low optical contrast achieved in the radiography image. However, the employment of standard digital processing techniques in the obtained image, is overcoming this disadvantage [7]. References [1] M. Lferde, Z. Lferde, M. Monnin, et al., Nucl. Tracks Radiat. Meas. 8 (1-4) (1984) 497. [2] R.L. Fleisher, P.B. Price, R.M. Walker, Nuclear Tracks in SolidsFPrinciple and Applications, University of California, Berkeley, California, 1975. [3] R. Ilic, M. Najzer, Nucl. Track Radiat. Meas. 17 (1990) 453. [4] R. Ilic, M. Najzer, Nucl. Track Radiat. Meas. 17 (1990) 461. [5] R. Ilic, M. Najzer, Nucl. Track Radiat. Meas. 17 (1990) 469. [6] R. Ilic, M. Najzer, Nucl. Track Radiat. Meas. 17 (1990) 475. [7] S.M.A. Pereira, M. Sc, Thesis, Nuclear Energy National Commission. IPEN-CNEN/SP Brazil, 2000. [8] Application Technology Information, The Makrolon 3200. Bayer AG, 1997. [9] R. Ilic, J. Rant, M. Humar, G. Somogyi, I. Hunyadi, Nucl. Tracks 12 (1-6) (1986) 933. [10] R. Antanasijevic, Z. Todorovic, A. Stamatovic, D. Miocinovic, Nucl. Instr. and Meth. 147 (1977) 139. [11] M.P.M. Assunc-a* o, R. Pugliesi, M.O. Menezes, Proceedings of the Fourth World Conference on Neutron Radiography, San Francisco, CA, USA, May 1992, pp. 10–16. [12] M.R. Hawkesworth, Atom Energy Rev. 152 (1977) 169. [13] M. Wrobel, L. Greim, Geesthacht, Germany, GKSS (1988) (GKSS 88/e/12). [14] A.A. Harms, A. Zellinger, Phys. Med. Biol. 22 (1) (1977) 70. [15] R. Pugliesi, M.A.S. Pereira, M.A.P.V. Moraes, M.O. Menezes, Appl. Radiat. Isot. 50 (1999) 375. [16] M.O. Menezes, M.Sc. Thesis, Nuclear Energy National Commission. IPEN-CNEN/SP Brazil, 1994.
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